Metal-organic frameworks (MOFs) are synthetic materials which can possess very high specific surface areas (e.g., exceeding 3000 m2/g). These high surface areas may make them useful for gas storage applications, for example, as hydrogen storage materials for fuel cell vehicles or methane storage materials for natural gas vehicles. The performance of these adsorbent materials may be highly dependent on the surface area based on the attraction of the gas to the surface due to Van Der Waals forces. Monolithic solids are generally superior for on-board gas storage applications (compared to powder) since they typically have greater total volumetric storage density, enhanced thermal properties, and improved ease of handling. However, bulk synthesis of MOFs generally results in a powder form of the material. It is possible to form MOFs into high-density pellets using mechanical compaction without a binder. However, mechanical compaction is known to reduce the micropore volume of the MOFs, due to pore collapse, pore blockage, and amorphization of crystal structure. This typically reduces the storage capacity of the MOFs, and limits the usefulness of densifying the MOF adsorbent.